diff --git a/test-typst/main.typ b/test-typst/main.typ index 5d49202..437fdb4 100644 --- a/test-typst/main.typ +++ b/test-typst/main.typ @@ -4,6 +4,7 @@ #show: super-T-as-transpose #set par.line(numbering: "1") +#set par(justify: true) // TODO: fix indent of first line #show figure.caption: it => { set text(10pt) @@ -48,6 +49,8 @@ // }) ) +#set heading(numbering: "1.") + = Introduction // SiC 是很好的材料。 @@ -111,19 +114,24 @@ experiment == Phonons in Perfect 4H-SiC +(There are 21 phonons in total. +We classified them into two categories: 18 negligible-polar phonons and 3 strong-polar phonons.) + // 拉曼活性的声子模式对应于 Gamma 点附近的声子模式。 // 根据这些声子模式的极性,我们将这些声子分成两类。 -Raman scattering peeks correspond to atom vibrations (phonons) located near the #sym.Gamma point in reciprocal space, - and the exact location of these phonons is determined by the wavevectors of incident and scattered light. -On each site of the Brillouin zone near the #sym.Gamma point, - there are 21 phonon modes in 4H-SiC. -We classified these phonons into two categories based on their polarities. -18 of 21 phonons are classified into negligible-polar phonons (i.e., phonons with zero or very weak polarity), +The phonons involved in Raman scattering are located in reciprocal space + at positions determined by the difference between the wavevectors of the incident and scattered light. +At each such position, there are 21 phonon modes (excluding translational modes). +We classify these 21 phonons into two categories based on their polarities. +The 18 of 21 phonons are classified into negligible-polar phonons (i.e., phonons with zero or very weak polarity), for which the effect of polarity can be ignored in the Raman scattering process; and the other three phonons are strong-polar phonons, where the polarity gives rise to observable effects in the Raman spectra. + +(This classification make sense.) + This classification is based on the fact that - the four Si atoms in the primitive cell carry similar positive Born effective charges (BECs), + the four Si atoms in the primitive cell of 4H-SiC carry similar positive Born effective charges (BECs), and the four C atoms carry similar negative BECs (see @table-bec). In the 18 negligible-polar phonons, the vibrations of two Si atoms are approximately opposite to those of the other two Si atoms, @@ -142,22 +150,21 @@ While in the three strong-polar phonons, table.cell(rowspan: 2)[C atom], [A/C layer], [-2.693], [-2.730], [B layer], [-2.648], [-2.800], ), - caption: [Born effective charges of Si and C atoms in A/B/C/B layers of 4H-SiC.], + caption: [ + Born effective charges of Si and C atoms in A/B/C/B layers of 4H-SiC, calculated using first principle method. + ], placement: none, ) === Phonons with Negligible Polarities -// 我们使用 Gamma 点的声子模式来近似拉曼过程中的非极性声子。 -// 这个近似被广泛使用,并且由于这个原因而被认为是可行的: -// 尽管拉曼过程中起作用的声子并不是那些严格在 Gamma 点的, -// 但这些声子模式的散射谱在 Gamma 附近连续且导数为零,且波矢很小(在本文中大约 0.01 A,只有c轴的大约2%)。 -// 因此,它们的性质与 Gamma 点的声子模式区别不大。 +(We investigate phonons at Gamma instead of the exact location near Gamma.) + Phonons at the #sym.Gamma point were used - to approximate negligible-polar phonons that participating in Raman processes. -This approximation is widely adopted and justified by the fact that, + to approximate negligible-polar phonons that participating in Raman processes of any incident/scattered light. +This approximation is widely adopted and justified by the fact that, // TODO: cite although the phonons participating in Raman processes are not these strictly located at the #sym.Gamma point, - their dispersion near the #sym.Gamma point is continuous with vanishing derivatives, + dispersion of negligible-polar phonons near the #sym.Gamma point is continuous with vanishing derivatives, and their wavevector is very small (about 0.01 nm#super[-1] in back-scattering configurations with 532 nm laser light, which corresponds to only 1% of the smallest reciprocal lattice vector of 4H-SiC), as shown by the orange dotted line in @figure-discont. @@ -182,43 +189,77 @@ Therefore, negligible-polar phonons involved in Raman processes placement: none, ) -// 这18个声子对应于 $\mathrm{C_{6v}}$ 点群的 14 个表示:2A1 + 4B1 + 2E_1 + 4E2 -// 其中,B1 表示没有拉曼活性,它的拉曼张量为零;其它表示的拉曼张量不为零 -// 但张量的大小是否足够大到可以在实验上看到,则还需要第一性原理计算,不能直接通过表示来判断。 -The 18 negligible-polar phonons correspond to 14 irreducible representations of the C#sub[6v] point group: - 2A#sub[1] + 4B#sub[1] + 2E#sub[1] + 4E#sub[2]. -Phonons belonging to A#sub[1] and B#sub[1] representations vibration along z-axis and are non-degenerate, - while phonons belonging to E#sub[1] and E#sub[2] representations vibrate in plane and are doubly degenerate. -Phonons belonging to B#sub[1] representation are Raman-inactive, as their Raman tensors vanish. -// TODO: 调整英语 -In contrast, phonons belonging to other representations are Raman-active, - and the non-zero components of Raman tensor of each phonon - could be determined by considering further in the C#sub[2v] point group @table-rep. -These Raman-active phonons might be visible in Raman experiment under appropriate polarization configurations. -However, the actual visibility of each phonon depends on the magnitudes of its Raman tensor components, - which cannot be computed solely from symmetry analysis. +(Representation of these 18 phonons, and the shape of their Raman tensors could be determined in advance.) + +Phonons of the B#sub[1] representation are Raman-inactive, as their Raman tensors vanish. +In contrast, phonons of the other representations are Raman-active, +and the non-zero components of their Raman tensors +can be determined by further considering the C#sub[2v] point group (see @table-rep). +These Raman-active phonons may appear in Raman spectra under appropriate polarization configurations. +However, the actual visibility of each mode depends on the magnitude of its Raman tensor components, +which cannot be determined solely from symmetry analysis. + +The 18 negligible-polar phonons correspond to 12 irreducible representations of the C#sub[6v] point group: + 2A#sub[1] + 4B#sub[1] + 2E#sub[1] + 4E#sub[2]. +Phonons belonging to the A#sub[1] and B#sub[1] representations vibrate along the z-axis and are non-degenerate, + while those belonging to the E#sub[1] and E#sub[2] representations vibrate in-plane and are doubly degenerate. +Phonons of the B#sub[1] representation are Raman-inactive, as their Raman tensors vanish. +In contrast, phonons of the other representations are Raman-active, + and the non-zero components of their Raman tensor + can be determined by further considering their representation in the C#sub[2v] point group (see @table-rep). +These Raman-active phonons might be visible in Raman experiment under appropriate polarization configurations. +However, whethear a mode is sufficiently strong to be experimentally visible + depends on the magnitudes of its Raman tensor components, + which cannot be determined solely from symmetry analysis. -// TODO: 完善表格 #figure({ let m2(content) = table.cell(colspan: 2, content); - table(columns: 7, align: center + horizon, inset: (x: 3pt, y: 5pt), - [*Rep in C6v*], [A#sub[1]], [B#sub[1]], m2[E#sub[1]], m2[E#sub[2]], - [*Rep in C2v*], [A#sub[1]], [B#sub[1]], [B#sub[2]], [B#sub[1]], [A#sub[2]], [A#sub[1]], - [*Vib Direction*], [z], [z], [x], [y], [x], [y], - [*Raman Tensor*], - [$mat(a, , ; , a, ; , , b)$], [$0$], [$mat( , , a; , , ; a, , ;)$], [$mat( , , ; , , a; , a, ;)$], - [$mat( , a, ; a, , ; , , ;)$], [$mat( a, , ; , -a, ; , , ;)$], - [*Raman Intensity*], - [$mat(a^2, , ; , a^2, ; , , b^2)$], [$0$], m2[$mat( , , a^2; , , a^2; a^2, a^2, ;)$], - m2[$mat( a^2, a^2, ; a^2, a^2, ; , , ;)$] + table(columns: 6, align: center + horizon, inset: (x: 3pt, y: 5pt), + [*Representations in C6v*], [A#sub[1]], m2[E#sub[1]], m2[E#sub[2]], + [*Representations in C2v*], [A#sub[1]], [B#sub[2]], [B#sub[1]], [A#sub[2]], [A#sub[1]], + [*Vibration Direction*], [z], [x], [y], [x], [y], + [*Raman Tensor of #linebreak() Individual Phonons*], + [$mat(a,,;,a,;,,b)$], [$mat(,,a;,,;a,,;)$], [$mat(,,;,,a;,a,;)$], [$mat(,a,;a,,;,,;)$], [$mat(a,,;,-a,;,,;)$], + [*Raman Intensity with Different #linebreak() Polarization Configurations*], + [xx/yy: $a^2$ #linebreak() zz: $b^2$ #linebreak() others: 0], + m2[xz/yz: $a^2$ #linebreak() others: 0], m2[xx/xy/yy: $a^2$ #linebreak() others: 0], )}, - caption: [Rep], + caption: [ + Raman-active representations of C#sub[6v] and C#sub[2v] point groups. + ], placement: none, ) -Here we propose a method to estimate the magnitudes of the Raman tensors of these phonons. +(We propose a method to estimate the magnitudes of the Raman tensors of these phonons. +Here we write out its main steps, details are in appendix.) -// TODO: 写出来这个方法,并验证。 +// TODO: maybe it is better to assign Raman tensor to each bond, instead of atom + +We propose a method to estimate the magnitudes of the Raman tensors by symmetry analysis (see appendix for details). + + +The center principle is to assign the Raman tensor (i.e., change of polarizability caused by atomic displacement) + to each atom in the unit cell. +This including the following steps: + - Write out the change of polarizability caused by displacement of Si atom in A and C layer, + Where unknown non-zero components are denoted by $a_1$, $a_2$, $a_5$, $a_6$. + For example, when we move the Si atom in A layer slightly towards the x+ direction in $d$ distance, + the change of polarizability should be $mat(,a_2,a_1;a_2,,;a_1,,)d$. + This could be done by conclusion above. + - The Si atom in B layer have similar local environment as the A and C layer, with only a little difference. + We denote these difference by $epsilon_1$, $epsilon_2$, $epsilon_5$, $epsilon_6$, + and the absolute value of $epsilon_i$ should be much smaller than $a_i$. + For example, when we move the Si atom in B layer slightly towards the x+ direction in $d$ distance, + the change of polarizability should be $mat(,a_2+epsilon_2,a_1+epsilon_1;a_2+epsilon_2,,;a_1+epsilon_1,,)d$. + - The local environment of C atom in A layer is similar to the Si atom in A layer with charge reversed and + the system reversed along xy plane. + We denote these difference by $eta_1$, $eta_2$, $eta_5$, $eta_6$, + and the absolute value of $epsilon_i$ should be much smaller than $a_i$. + For example, when we move the C atom in A layer slightly towards the x+ direction in $d$ distance, + the change of polarizability should be $mat(,a_2+eta_2,-a_1-eta_1;a_2+eta_2,,;-a_1-eta_1,,)d$. + - Similar to the case in Si atoms, we derive the change of polarizability + caused by moving C atom in B layer slightly towards the x+ direction in $d$ distance, + which should be $mat(,-a_2-eta_2-zeta_2,-a_1-eta_1-zeta_1;-a_2-eta_2-zeta_2,,;-a_1-eta_1-zeta_1,,)d$. Lets assign Raman tensor onto each atom. That is, Raman tensor is derivative of the polarizability with respect to the atomic displacement: @@ -379,6 +420,11 @@ No. It turns out to be similar to the C atom in C layer. We summarize these stuff into @table-singleatom. Furthermore, we list predicted modes and their Raman tensors, in @table-predmode. +- $a$: Raman tensor of Si atom in A layer, large value. +- $epsilon$: Difference of Raman tensors of Si atom in A and B1 layer, small value. +- $eta$: Difference of Raman tensors of C and Si atom in A layer, small value. +- $zeta$: Difference of Raman tensors of C atoms in A and B layer, small value. + Frequency could be estimated by, how many atoms are moving towards its neighbor. #page(flipped: true)[#figure({ @@ -444,39 +490,6 @@ Frequency could be estimated by, how many atoms are moving towards its neighbor. placement: none, )] - -/* -这里应该有办法来估计。下面是我总结的规律: -按照我们规定的 ABCB 层序,并将拉曼张量的大小归结为键长的变化的话: -* 对于 E2 表示(AC层运动方向必须相反,B1/B2层运动方向必须相反,因此只讨论A和B1层) - * A 层内部的那个竖的键,同向运动会导致比较大的拉曼张量 - * B1 层内部的那个竖的键,反向运动会导致比较大的拉曼张量 - * A 层和 B1 层之间的那个横的键,反向运动会导致比较大的拉曼张量 -我们或许可以通过这个路径来探索: -* 首先,根据 C3v 点群的表示,写出每个键的拉曼张量。这包括: - * 对于 A 内竖着的键,考虑连着的两个原子和第一近邻原子,对称性为 C3v。写出此时的拉曼张量。 - * 对于 B1 内竖着的键,它也是 C3v,它此时的拉曼张量是 h 下稍微变动的结果。写下这个结果。 - * 对于 A 到 B1 的横着的键,它是 C3v 。写下这个结果。 - * 对于 B1 到 C 的横着的键,它是 C3v 。写下这个结果为之前的结果的微微变动。 - * 对于其它键,根据对称性由上面的结果直接写出。 -* 写出各个模式的拉曼张量(上面的线性组合)。即可以直接看到结果。 -*/ -// -// 考虑 A 层的竖着的键。面内的振动模式对应的拉曼张量落在两个空间中。 -// 在第一个空间中,它的形式为: -// -// $ -// mat(a, , ; , -a, ; , , ;) -// mat(, a, ; a, , ; , , ;) -// $ -// -// 在第二个空间中,它的形式为: -// -// $ -// mat(, , a; , , ; a, , ;) -// mat(, , ; , , a; , a, ;) -// $ - // 我们计算了拉曼活性声子的频率及拉曼张量,并与实验对比,如表如图所示。 // 其中有几个声子的拉曼活性较弱,有几个比较强。强的都可以在实验上看到;但弱的能否看到则取决于它是否恰好位于强模式的附近。 // 其中,xxx 和xxx 位于强模式的附近,它们在实验上无法看到;xxx 只在 z 方向入射/散射时可以看到;xxx 则在任意方向都能看到。